Affiliation:
1. Laboratoire de Chimie Théorique, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, QC J1K 2R1, Canada.
Abstract
The nonlinear nonperturbative response of OCS and CS2 to ultrashort (few cycles) intense laser pulses was studied numerically by time-dependent density functional theory (TDDFT) methods to understand molecular ionization as a function of laser–molecule orientation. A time-dependent electron localization function(TDELF) was used to visualize the nonlinear nonperturbative electron transfer occurring during the laser pulse. It was found that, for intensities I > 3.5 × 1014 W/cm2, the inner shell Kohn–Sham (KS) molecular orbitals contribute significantly to the ionization, whereas for the intensity I < 3.5 × 1014 W/cm2, the highest occupied molecular orbital (HOMO) shows the dominant response to the field. In general, the ionization rate maxima correspond to the alignment of maximum KS orbital densities with the laser pulse polarization instead of orbital ionization potentials (IP). These findings are corroborated through analysis of the TDELF images, where the ionization occurs from the lone pair or bond regions of the corresponding molecules.
Publisher
Canadian Science Publishing
Subject
Organic Chemistry,General Chemistry,Catalysis
Reference34 articles.
1. Intense few-cycle laser fields: Frontiers of nonlinear optics
2. Attosecond physics
3. Observing electron motion in molecules
4. Ullrich, C. A.; Bandrauk, A. D. In Time-Dependent Density Functional Theory; Marques, M. A. L.; Nogueira, F.; Rubio, A.; Burke, K.; Ullrich, C.A.; Gross, E. K. U., Eds.; Springer: Berlin, 2006; pp 357–374.
5. Nonlinear time-dependent density-functional-theory study of ionization and harmonic generation in CO2by ultrashort intense laser pulses: Orientational effects
Cited by
4 articles.
订阅此论文施引文献
订阅此论文施引文献,注册后可以免费订阅5篇论文的施引文献,订阅后可以查看论文全部施引文献